Abstract Discontinuous solid-solid phase transformations play a pivotal role in determining the properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in LixNi0.5Mn1.5O4within an operational Li metal coin cell. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to a planar semi-coherent interface driven by dislocation dynamics. Our data indicates negligible kinetic limitations from interface propagation impacting the transformation kinetics, even at a discharge rate of C/2 (80 mA/g). This study highlights BCDI’s capability to decode complex operando diffraction data, offering exciting opportunities to study nanoscale phase transformations with various stimuli.
more »
« less
Generation of high-order harmonics and attosecond pulses in the water window via nonlinear propagation of a few-cycle laser pulse
We theoretically and computationally study the generation of high-order harmonics in the water window from a semi-infinite gas cell where a few-cycle, carrier-envelope-phase-controlled 1.7-µm driving laser pulse undergoes nonlinear propagation via optical Kerr effect (self-focusing) and plasma defocusing. Our calculation shows that high harmonic signals are enhanced for extended propagation distances and furthermore, isolated attosecond pulses in the water window can be generated from the semi-infinite gas cell. This enhancement is attributed mainly to better phase matching for extended propagation distances achieved via nonlinear propagation and resulting intensity stabilization.
more »
« less
- PAR ID:
- 10518801
- Publisher / Repository:
- Optica
- Date Published:
- Journal Name:
- Optics Express
- Volume:
- 31
- Issue:
- 20
- ISSN:
- 1094-4087
- Page Range / eLocation ID:
- 32488
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Context.Acetone (CH3COCH3) is one of the most abundant three-carbon oxygen-bearing complex organic molecules (O-COMs) that have been detected in space. The previous detections were made in the gas phase toward star-forming regions that are chemically rich, mostly in protostellar systems. Recently, acetone ice has also been reported as (tentatively) detected toward two low-mass protostars, allowing comparisons in acetone abundances between gas and ice. The detection of acetone ice warrants a more systematic study of its gaseous abundances which is currently lacking. Aims.We aim to measure the gas-phase abundances of acetone in a large sample obtained from the CoCCoA program, and investigate the chemical evolution of acetone from ice to gas in protostellar systems. Methods.We fit the ALMA spectra to determine the column density, excitation temperature, and line width of acetone in 12 high-mass protostars as part of CoCCoA. We also constrained the physical properties of propanal (C2H5CHO), ketene (CH2CO), and propyne (CH3CCH), which might be chemically linked with acetone. We discuss the possible formation pathways of acetone by making comparisons in its abundances between gas and ice and between observations and simulations. Results.We firmly detect acetone, ketene, and propyne in the 12 high-mass protostars. The observed gas-phase abundances of acetone are surprisingly high compared to those of two-carbon O-COMs (especially aldehydes). Propanal is considered as tentatively detected due to lack of unblended lines covered in our data. The derived physical properties suggest that acetone, propanal, and ketene have the same origin from hot cores as other O-COMs, while propyne tends to trace the more extended outflows. The acetone-to-methanol ratios are higher in the solid phase than in the gas phase by one order of magnitude, which suggests gas-phase reprocessing after sublimation. There are several suggested formation pathways of acetone (in both ice and gas) from acetaldehyde, ketene, and propylene. The observed ratios between acetone and these three species are rather constant across the sample, and can be well reproduced by astrochemical simulations. Conclusions.On the one hand, the observed high gas-phase abundances of acetone along with dimethyl ether (CH3OCH3) and methyl formate (CH3OCHO) may hint at specific chemical mechanisms that favor the production of ethers, esters, and ketones over alcohols and aldehydes. On the other hand, the overall low gas-phase abundances of aldehydes may result from destruction pathways that are overlooked or underestimated in previous studies. The discussed formation pathways of acetone from acetaldehyde, ketene, and propylene seem plausible from observations and simulations, but more investigations are needed to draw more solid conclusions. We emphasize the importance of studying acetone, which is an abundant COM that deserves more attention in the future.more » « less
-
In this work, we show that collisions of one type of nonlinear wave can lead to generation of a different kind of nonlinear wave. Specifically, we demonstrate the formation of topological solitons (or transition waves) via collisions of elastic vector solitons, another type of nonlinear wave, in a multistable mechanical system with coupling between translational and rotational degrees of freedom. We experimentally observe the nucleation of a phase transformation arising from colliding waves, and we numerically investigate head-on and overtaking collisions of solitary waves with vectorial properties (i.e., elastic vector solitons). Unlike KdV-type solitons, which maintain their shape despite collisions, our system shows that collisions of two vector solitons can cause nucleation of a new phase via annihilation of the vector solitons, triggering the propagation of transition waves. The propagation of these depends both on the amount of energy carried by the vector solitons and on their respective rotational directions. The observation of the initiation of transition waves with collisions of vector solitons in multistable mechanical systems is an unexplored area of fundamental nonlinear wave interactions and could also prove useful in applications involving reconfigurable structures.more » « less
-
Abstract High-eccentricity gas giant planets serve as unique laboratories for studying the thermal and chemical properties of H/He-dominated atmospheres. One of the most extreme cases is HD 80606 b—a hot Jupiter orbiting a Sun-like star with an eccentricity of 0.93—which experiences an increase in incident flux of nearly 3 orders of magnitude as the star–planet separation decreases from 0.88 au at apoastron to 0.03 au at periastron. We observed the planet’s periastron passage using JWST’s NIRSpec/G395H instrument (2.8–5.2μm) during a 21 hr window centered on the eclipse. We find that, as the planet passes through periastron, its emission spectrum transitions from a featureless blackbody to one in which CO, CH4, and H2O absorption features are visible. We detect CH4during postperiapse phases at 4.1–10.7σdepending on the phase and on whether a flux offset is included to account for NRS1 detector systematics. Following periapse, H2O and CO are also detected at 4.2–5.5σand 3.7–4.4σ, respectively. Furthermore, we rule out the presence of a strong temperature inversion near the IR photosphere based on the lack of obvious emission features throughout the observing window. General circulation models had predicted an inversion during periapse passage. Our study demonstrates the feasibility of studying hot Jupiter atmospheres using partial phase curves obtained with NIRSpec/G395H.more » « less
-
Abstract The dominant form of oxygen in cold molecular clouds is gas-phase carbon monoxide (CO) and ice-phase water (H2O). Yet, in planet-forming disks around young stars, gas-phase CO and H2O are less abundant relative to their interstellar medium values, and no other major oxygen-carrying molecules have been detected. Some astrochemical models predict that gas-phase molecular oxygen (O2) should be a major carrier of volatile oxygen in disks. We report a deep search for emission from the isotopologue16O18O (NJ= 21− 01line at 233.946 GHz) in the nearby protoplanetary disk around TW Hya. We used imaging techniques and matched filtering to search for weak emission but do not detect16O18O. Based on our results, we calculate upper limits on the gas-phase O2abundance in TW Hya of (6.4–70) × 10−7relative to H, which is 2–3 orders of magnitude below solar oxygen abundance. We conclude that gas-phase O2is not a major oxygen carrier in TW Hya. Two other potential oxygen-carrying molecules, SO and SO2, were covered in our observations, which we also do not detect. Additionally, we report a serendipitous detection of the C15NNJ= 25/2− 13/2hyperfine transitions,F= 3 − 2 andF= 2 − 1, at 219.9 GHz, which we found via matched filtering and confirm through imaging.more » « less
An official website of the United States government

